The synthesis of efficient, stable, and green multifunctional electrode materials is a long-standing challenge for modern society in the field of energy storage and conversion. To this end, we successfully synthesized five bimetallic precursor materials with excellent performance by hydrothermal reaction with the assistance of a high concentration of polyvinylpyrrolidone (PVP), and then, sulfide etched the lamellar precursor materials among them to obtain the one-dimensional heterostructured samples. Benefiting from the synergistic effect of the bimetal and the continuous electron/ion transport structure, the samples displayed excellent bifunctional activity in supercapacitor and oxygen evolution reaction (OER). Regarding supercapacitors, the exceptional performance of 2817.2 F g−1 at 1 A g−1 was demonstrated, while the asymmetric supercapacitors made showed an extraordinary energy density of 150.2 Wh kg−1 at a power density of 618.5 W kg−1 and outstanding cycling performance (94.74% capacity retention after 20,000 cycles at 10 A g−1). Simultaneously, a wearable flexible electrode that can be wrapped around a finger was coated on a carbon cloth and was found to light up a 0.5-m-long strip of light. Moreover, it exhibited an ultralow oxygen reduction overpotential of 249 mV at 10 mA cm−2. Hence, our work provides a facile strategy to modulate the synthesis of heterogeneous structured sulfides with a continuous electron/ion transport pathway, which possesses excellent oxygen reduction electrocatalytic performance while meeting superior supercapacitor performance. Such work provides an effective approach for the construction of multifunctional electrochemical energy materials.